Proton switching molecular magnetoelectricity

Yong Hu; Scott Broderick; Zipeng Guo; Alpha T N'Diaye; Jaspal S Bola; Hans Malissa; Cheng Li; Qiang Zhang; Yulong Huang; Quanxi Jia; Christoph Boehme; Z Valy Vardeny; Chi Zhou; Shenqiang Ren

doi:10.1038/s41467-021-24941-9

Proton switching molecular magnetoelectricity

Nat Commun. 2021 Jul 29;12(1):4602. doi: 10.1038/s41467-021-24941-9.

Authors

Yong Hu¹, Scott Broderick², Zipeng Guo³, Alpha T N'Diaye⁴, Jaspal S Bola⁵, Hans Malissa⁵, Cheng Li⁶, Qiang Zhang⁶, Yulong Huang¹, Quanxi Jia², Christoph Boehme⁵, Z Valy Vardeny⁵, Chi Zhou³, Shenqiang Ren^{7

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Affiliations

¹ Department of Mechanical and Aerospace Engineering, University at Buffalo, The State University of New York, Buffalo, NY, USA.
² Department of Materials Design and Innovation, University at Buffalo, The State University of New York, Buffalo, NY, USA.
³ Department of Industrial and Systems Engineering, University at Buffalo, The State University of New York, Buffalo, NY, USA.
⁴ Advanced Light Source (ALS), Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
⁵ Department of Physics & Astronomy, University of Utah, Salt Lake City, UT, USA.
⁶ Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA.
⁷ Department of Mechanical and Aerospace Engineering, University at Buffalo, The State University of New York, Buffalo, NY, USA. shenren@buffalo.edu.
⁸ Department of Chemistry, University at Buffalo, The State University of New York, Buffalo, NY, USA. shenren@buffalo.edu.
⁹ Research and Education in Energy Environment & Water Institute, University at Buffalo, The State University of New York, Buffalo, NY, USA. shenren@buffalo.edu.

Abstract

The convergence of proton conduction and multiferroics is generating a compelling opportunity to achieve strong magnetoelectric coupling and magneto-ionics, offering a versatile platform to realize molecular magnetoelectrics. Here we describe machine learning coupled with additive manufacturing to accelerate the design strategy for hydrogen-bonded multiferroic macromolecules accompanied by strong proton dependence of magnetic properties. The proton switching magnetoelectricity occurs in three-dimensional molecular heterogeneous solids. It consists of a molecular magnet network as proton reservoir to modulate ferroelectric polarization, while molecular ferroelectrics charging proton transfer to reversibly manipulate magnetism. The magnetoelectric coupling induces a reversible 29% magnetization control at ferroelectric phase transition with a broad thermal hysteresis width of 160 K (192 K to 352 K), while a room-temperature reversible magnetic modulation is realized at a low electric field stimulus of 1 kV cm^-1. The findings of electrostatic proton transfer provide a pathway of proton mediated magnetization control in hierarchical molecular multiferroics.

Abstract

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